Gold nanocrystals passivated by self‐assembled monolayers of straightchain alkylhiolate molecules have been obtained as highly purified molecular materials of high intrinsic stability. Evidence is presented for a predicted discrete sequence of energetically optimal fcc structures of a truncated octahedral morphological motif (see cover). The nanocrystal materials have a propensity to form extended superlattics, such as that in the Figure.

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